跳到主要內容

臺灣博碩士論文加值系統

(44.192.20.240) 您好!臺灣時間:2024/02/24 23:06
字體大小: 字級放大   字級縮小   預設字形  
回查詢結果 :::

詳目顯示

: 
twitterline
研究生:錢信丞
研究生(外文):Shin-Cheng Chien
論文名稱:斗六地區PM2.5酸性氣膠特徵之研究
論文名稱(外文):The acid aerosols characteristics of PM2.5 particle in Dauliou , Yunlin
指導教授:李經民李經民引用關係
指導教授(外文):James J. Lee
口試委員:鄭曼婷陳瑞仁周崇光李經民
口試委員(外文):Man-Ting , ChengRuei-Ren ,ChenChung-Kuang ,ChouJames J. Lee
口試日期:2014-07-25
學位類別:碩士
校院名稱:國立雲林科技大學
系所名稱:環境與安全衛生工程系
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2014
畢業學年度:102
語文別:中文
論文頁數:68
中文關鍵詞:懸浮微粒酸性氣膠生質燃燒衍生型氣膠
外文關鍵詞:PM2.5acid aerosolbiomass burningSecondary areosolNear-source
相關次數:
  • 被引用被引用:5
  • 點閱點閱:876
  • 評分評分:
  • 下載下載:26
  • 收藏至我的研究室書目清單書目收藏:0
依據環保署資料顯示雲林縣PM2.5平均濃度居全台前三名,縣內以斗六站濃度最高,故討論斗六地區PM2.5特性有其必要性。本研究使用高流量與環形擴散(Annular Denuder Sampler,ADS )採樣器探討近兩年(2012-2013) 斗六地區PM2.5,及其陰陽離子、脫水葡萄糖、氣/固相污染物之季節化學特徵。
研究結果顯示斗六地區PM2.5平均濃度以秋、冬季最高 (48.8、63.5 μg/m3) 、春季次之(50.4 μg/m3),夏季濃度最低(32.7 μg/m3)。秋冬季節斗六位於季風背風面,大氣擴散不良氣膠容易老化PM濃度上升;春季PM2.5變異性較大,高濕度環境(如春季晨霧)容易形成衍生型氣膠使PM2.5濃度升高。PM2.5日/夜比值方面,以冬季夜間濃度比值最高(日/夜,0.66),可能因冬季日間光化反應、夜間高濕度有利於夜間PM2.5衍生性氣膠形成;其他季節則是日間濃度大於夜間。其次,由脫水葡萄醣濃度瞭解生質燃燒對大氣PM2.5貢獻量,數據顯示夏冬季稻作燃燒佔大氣PM2.5貢獻二成左右,顯示每年夏冬季稻作生質燃燒為斗六地區PM2.5主要污染來源之一。離子方面,以硫酸鹽、硝酸鹽、及銨鹽等衍生型氣膠為PM2.5主要成份;離子季節分佈以秋冬兩季濃度最高,可能因季風期間大氣擴散不良與污染物累積有關。其中NO3-濃度隨季節性變化較明顯,冬季濃度是夏季的五倍,可能NH4NO3在低溫環境下較不利揮發有關。SO42-除夏季濕沉降使其濃度下降外,其餘三季硫酸鹽濃度較高(~10 μg/m3)。
斗六地區大氣氣相污染物(氣相僅量測2013夏秋冬三個季節)主要成份包含: NH3、SO2、HNO2、及HNO3,三季平均濃度分別為16.39、6.18、3.89、1.05ppbv。其中秋、冬季節(旱季)有較高濃度的NH3、HNO2氣相污染物,夏季因溼沉降洗滌使其濃度值下降。高濃度NH3可能因雲林畜牧養殖較多有關(如雲林養豬全台第一 ~140萬頭);而NH3又是PM2.5衍生氣膠前驅物質,HNO2則是大氣氫氧自由基最主要來源之一,故此兩種氣相物質未來仍應進行持續的研究。氣/固相分佈方面,斗六冬季的氣相與固相污染物濃度皆高(氣/固比值 0.98);但秋季氣相濃度卻明顯高於固相濃度(氣/固比值 2.02,氣相濃度是固相2倍),其粒子也呈現有高濃度的生質燃燒指標物( Levo, 227ng/m3 ),顯示秋季氣相污染物可能來自上風處(東北風)生質燃燒污染氣團有關。 本研究初步結果顯示斗六地區秋冬季節具有高濃度的氣相污染物,涉及PM2.5衍生氣膠前驅物與大氣高氧化性來源(氫氧自由基),故斗六大氣氣/固相分佈研究,仍有待持續的進行調查與釐清原因,以供日後相關研究參考之用。

The data of ROC EPA indicates the PM2.5 concentration of Douliou monitoring station in Yunlin County ranked the top three counties in Taiwan in recent years. so It is necessity to discussion Douliou regional PM2.5 characteristics. In this study, the use high volum flow and annular diffusion (Annular Denuder Sampler, ADS) sampler explore PM2.5、ions、Anhydro sugar、gas / solid phase pollutants at Douliou area in past two years. (2012-2013)
In Douliou region the average concentration of PM2.5 in autumn and winter are the highest (48.8~63.5 μg/m3), spring are secondary (50.4μg/m3), the lowest is summer (32.7μg/m3). Douliou located leeward area and poor atmospheric dispersion could rise PM2.5 aerosol concentration easily in fall and winter season; PM2.5 concentrations are variable in Spring, high-humidity environment (such as morning fog) is easy to yield secondary PM2.5 aerosol concentration. The PM2.5 Day/Night ratio is the highest concentrations in winter night(day/night,0.66), probably due to photochemical reactions in winter day time, night time high humidity favor the formation of PM2.5 secondary aerosol; other seasons are daytime concentrations greater than the night. By levoglucosan concentration to predict the contribution of biomass burning on atmospheric PM2.5. Summer and winter rice burning contribute around 20% of atmospheric PM2.5 contribution, showing the summer and winter rice biomass burning for Douliou area PM2.5 one of the main sources of pollution. The main components of PM2.5 is sulfate、nitrate and ammonium salts. The highest ion concentration in autumn and winter season may be due to poor atmospheric dispersion and pollutants accumulate during the northeast seasonal wind. NO3- concentration with obvious seasonal variation. Winter concentration is five times than summer at lower temperature may NH4NO3 volatilization less favorable. SO42- low concentration in summer due to wet deposition drops, the other season of high sulfate concentrations (~ 10 μg /m3).
The average gas pollutants concentrations NH3、SO2、HNO2、and HNO3 is 16.39,6.18,3.89,1.05ppbv in Douliou (measure 2013 summer autumn three seasons). The higher concentrations of NH3、HNO2 gas pollutants in autumn and winter. The lower concentration in summer due to wet deposition decline concentration. High concentrations of NH3 may be more relevant livestock at Yunlin (Taiwan's first cloud forest hog ~ 1.4 million). NH3 is PM2.5 secondary aerosol precursors, HNO2 is atmospheric hydroxyl radical in the most one of the main sources. Those gas material should concerned in the future. Gas / solid phase pollutant concentrations are higher in winter (gas / solid ratio of 0.98); but autumn gas concentration was higher than particle concentration (gas / solid ratio of 2.02), its particle biomass burning indicators Levoglucosan showed a high concentration (Levo, 227ng/m3). The pollution may come from upwind (northeast) related to biomass burning in fall season. In this study show high concentrations gas pollutants, involving PM2.5 secondary aerosol and atmospheric aerosol precursors highly oxidizing source (hydroxyl radical) in fall and winter at Douliou areas. Douliu atmospheric gas / solid phase distribution research remains to be continuing to investigate and clarify the reasons for the research reference in the future.


中文摘要 i
Abstract ii
誌謝 iii
目錄 iv
表目錄 vi
圖目錄 vii
第一章 前言 1
第二章文獻回顧 3
2-1懸浮微粒來源與物化特性 3
2-2 硫酸銨及硝酸銨之形成機制 3
2-3 PM2.5酸性氣膠之相關研究 5
2-4硝酸與亞硝酸氣相污染物之形成機制 6
2-5 生質燃燒脫水醣的應用 8
第三章 研究方法 11
3-1 採樣設備 11
3-1-1 傳統二階採樣器 11
3-1-2 環形擴散採樣器( Annular Denuder System,ADS ) 12
3-2 採樣地點與條件 13
3-3 採樣前準備 14
3-3-1 濾紙前處理 14
3-3-2環形擴散採樣器( Annular Denuder System,ADS ) 氣體吸附管 14
3-4 化學分析方法 15
3-4-1 採樣濾紙萃取 15
3-4-2化學成分分析 16
3-5 分析方法品保/品管 ( QA/QC ) 17
3-5-1 分析化合物檢量線製作 18
3-5-2 方法偵測極限測定 ( MDL ) 18
3-5-3 回收率 ( Recovery ) 19
3-5-4 再現性 ( Reproducibility ) 19
3-5-5 空白樣本分析 ( Blank ) 20
第四章 結果與討論 25
4-1大氣氣象與PM氣膠濃度解析 25
4-2水溶性陰陽離子特徵 28
4-2-1水溶性陰陽離子當量比值 28
4-2-2水溶性陰陽離子濃度 29
4-3生質燃燒與事件日之特徵探討 32
4-4氣、固相污染物特徵分布之探討 34
4-4-1氣相污染物濃度 34
4-4-2 Near-source 與生質燃燒指標HNO2 (氣相)、Levo (固相)之關係 37
第五章 結論與建議 58
5-1結論 58
5-2建議 60
參考文獻 61
附錄 66


1.Appel B. R., 1993,“Atmospheric sample analysis and sampling artifacts. Aerosolmeasurement : principles, techniques, and applications”, New York, NY . VanNostrandReinhold, pp.233-259.

2.Aumont, B., F. Chervier and S. Laval,2003, “Contribution of HONO Sources to the NOx/HOx/O3 Chemistry in the Polluted Boundary Layer,” Atmospheric Environment, Vol. 37, No. 4, pp. 487-498.

3.Baltensperger U., 1997.Analysis of aerosols. Chimia vol.51 (10),pp.686- 689.

4.Brook, J. R., T. F. Dann and R. T. Burnett, 1997,“The Relationship Among TSP, PM10, PM2.5, and Inorganic Constituents of Atmospheric Particulate Matter at Multiple Canada Locations,”J. Air & Waste Manage. Assoc., Vol. 47, pp. 2-19.

5.Biswas K.F.,Ghauri B.M.,and Husain L., 2008, “Gaseous and aerosol pollutants during fog and clear episodes in South Asian urban atmosphere”, Atmospheric Environment , vol.42, pp.7775-7785.

6.Bytnerowicz A.,Tausz M.,Alonso R.,Jones D.,Johnson R., and Grulke N.,2002, “Summer-time distribution of air pollutants in Sequoia national park , California”, Evironmental Pollution , vol.118 , pp.187-203.

7.Colbeck I. And R. M. Harrison ,1984, “Ozone-Secondary Aerosol-Visibility Relationships in North-West England,” The Science of Total Environment, Vol. 34, pp. 87-100.

8.Danalatos D. and S. Glavas, 1995, ”Atmospheric Nitric Acid Concentrations in a Mediterranean site, Patras, Greece,” Atmospheric Environments Vol. 29 No.15, pp. 1849-1852 .

9.Fraser M.P., and Lakshmanan K., 2000, “Using levoglucosan as a molecular marker for the long-range transport of biomass combustion aerosols”,Environmental Science and Technology, vol. 34, pp. 4560-4564

10.Graedel T.E., and Keene W.C., 1996, “The budget and cycle of Earth’s natural Chlorine”, Pure & Appl. Chem., vol.68, pp.1689-1697.

11.Gutzwiller, L., F. Arens, U. Baltensperger, H. W. Gaggeler and M. Ammann,2002, “Signification of Semivolatile Diesel Exhaust Organics for Secondary HONO Formation,” Environment Sciences & Technology, Vol. 36, No. 4, pp. 677-682.

12.Harrison, R. M. and A. M. N. Kitto,1994, “Evidence for a Surface Source of Atmospheric Nitrous Acid,” Atmospheric Environment, Vol. 28, No. 6, pp. 1089-1094.

13.Harrison, A., B. Bessagnet and R. Vautard,1997, “A Model Evaluation of Coarse -Mode Nitrate Heterogeneous Formation on Dust Particles,” Atmospheric Environment, Vol. 40, pp. 4158-4171 .

14.Hennigan C.J., Sullivan A.P., Collett Jr., J.L., and RobinsonA.L.,2010, “Levoglucosan stability in biomass burning particles exposed to hydroxyl radicals”, Geophysical Research Letters, vol. 37, pp. L09806.

15.Hinds W.C., 1997, Properties, behavior and measure of airborne particles, 2nd edition.Aerosol Technology, New York, USA.pp.3-4.

16.Hoffmann D., Tilgner A., Iinuma Y., and Herrmann H., 2010, “Atmospheric stability of levoglucosan: A detailed laboratory and modeling study”, Environmental Science and Technology, vol. 44, pp. 694-699.

17.Lee H. S., C. M. Kang, B. W. Kang, and H. K. Kim,1999, ”Seasonal Variations of Acidic Pollutants in Seoul, South Korea,” Atmospheric Environment Vol. 33 , pp.3143-3152.

18.Lin, Y. C., M. T. Cheng, W. Y. Ting and C. R. Yeh,2006, “Characteristics of Gaseous HNO2, HNO3, NH3 and Particulate Ammonium Nitrate in an Urban City of Central Taiwan,” Atmospheric Environment, Vol. 40, pp. 4725-4733.

19.Kang C.M.,Lee H.S.,Kang B.W.,Lee.K.,and SunwooY.,2004,“Chemical characteristics of acidic gas pollutants and PM2.5 species during hazy episodes in Seoul, South Korea”, Atmospheric Environment ,vol.38, pp. 4749-4760.

20.Khoder M.I.,2002, “Atmospheric conversion of sulfur dioxide to particulate sulfate and nitrogen dioxide to particulate nitrate and gaseous nitric acid in an urban area”,Air Pollution Department, vol.49,pp. 675-684.

21.Kurtenbach, R., K. H. Becker, J. A. G. Gomes, J. Klrffmann, J. C. Lorzer, M. Spittler, P. Wiesen, R. Ackermann, A. Geyer and U. Platt, 2001,“Investigations of Emissions and Heterogeneous Formation of HONO in a Road Traffic Tunnel,” Atmospheric Environment, Vol. 35, pp. 3385-3394.

22.Lee S.H., Kang C.M., Kang B.W., and Kim H.K.,1999, “ Seasonal variations of acidic air pollutants in Seoul, South Korea” , Atmospheric Environment, vol.33, pp.3143-3151.

23.Leitheada A., Lia S.M, Hoffb R, Chenga Y, and Brook J, 2006, “Levoglucosan and dehydroabietic acid: Evidence of biomass burning impact on aerosols in the Lower Fraser Valley”, Atmospheric Environment, vol.40, pp.2721-2734.

24.Lippmann M., 1989, “Background on health effects of acid aerosols”, Environment Health Perspect, vol.79, pp.3-6.

25.Matsumoto K. and H. Tanaka, 1996 ,“Formation and dissociation of atmospheric particulate Nitrate and Chloride : an approach based on phase equilibrium” ,Atmospheric Environment, vol. 30, pp. 639-648.

26.Matsumoto M. and T. Okita,1998,”Long Term Measurements of Atmospheric Gaseous Aerosol Species Using an Annular Denuder System in Nara, Japan,” Atmospheric Environment Vol. 32 ,No. 8, pp.1419-1425.

27.Mozurkewich M., 1993, “The dissociation constant of Ammonium Nitrate and its dependence on temperature, relative humidity and particle size”, Atmospheric Environment, vol. 27a, pp. 261 - 270.

28.Na, K., A. A. Sawant, S. Chen and D. A. Cocker Ⅲ,2004, “Primary and Secondary Carbonaceous Species in the Atmosphere of Western Riverside County, California,” Atmospheric Environment, Vol. 38, pp. 1345-1355.

29.Ohta, S. and T. Okita,1990, “A Chemical Characterization of Atmospheric Aerosol in Sapporo,” Atmospheric Environment, Vol. 24A, No. 4, pp. 815-822 .

30.Pashynska V.,Vermeylen R.,Vas G., Maenhaut W., and Claeys M., 2002, “Development of a gas chromatography/ion trap mass spectrometry method for determination of levoglucosan and saccharidic compounds in atmospheric aerosol. Application to urban arosol” ,Journal of Mass Spectrom, vol.37,pp.1249-1257.

31.Qin, Y., E. Kim and P. K. Hopke, 2006,“The Concentrations and Sources of PM2.5 in Metropolitan New York City,” Atmospheric Environmental, Vol. 40, pp. 312-332.

32.Qin M., Xie P., Su H., Gu J., Peng F., Li S., Zeng L., Liu J., Liu W.,and Zhang Y., 2009, “An observational study of the HONO–NO2 coupling at an urban sitein Guangzhou City, South China”, vol.43, pp.5731-5742.

33.Ren X., Harder H., Martinez M., Lesher R., Oliger A., Simpas J., Brune W., Schwab J., Demerjian K., He Y., Zhou X., and Gao H., 2003 ,“OH and HO2 Chemistry in the urban atmosphere ofNew York city”, Atmospheric Environment,vol.37, pp.3639-3651.

34.Seinfeld J. H. and Pandis S. N., 1998, “Atmospheric chemistry and physics from air pollution to climate change,” John Wiley & Sons, Inc., New York.

35.Seinfeld, J. H. and S. N. Pandis., Atmospheric Chemistry and Physics, Wiley, New York, pp. 234-336(1998).

36.Stelson, A.W., Seinfeld, J.H., 1982a., “Relative humidity and temperature dependence of the ammonium nitrate dissociation constant. ”, Atmospheric Environment, 16(5), pp.983-992.

37.Stelson, A.W., Seinfeld, J.H., 1982b., “Thermodynamic prediction of the water activity, ammonium nitrate dissociation constant ,density and refractive index for the ammonium nitrateammonium sulfate-water systema at 25°C., Atmospheric Environment (1967-1989)16 (10), pp.2507-2514.

38.Stelson A.W., Seinfeld J.H.., 2007., “Relative humidity and temperature dependence of the ammonium nitrate dissociation constant Atmos. ” Environ., 41 (Suppl.), pp. 126–135

39.Simoneit B.R.T., Schauer J.J., Nolte C.G., Oros D.R., Elias V.O., Fraser M.P., Rogge W.F., and Cass G.R., 1999, “Levoglucosan, a tracer for cellulose in biomass burning and atmospheric particles”, Atmospheric Environment, vol.33, pp.173-182.

40.Simoneit B.R.T., and Elias, V.O., 2000, “Organic tracers from biomass burning in atmospheric particulate matter over the ocean”, Marine Chemistry, vol. 69, pp. 301-312.

41.Sioutas C., Wang P.Y.,Ferguson S.T., and Koutrakis P., 1996; “Laboratory and field evaluation of an improved glass honeycomb denuder/filter pack sampler,” Atmospheric Environment., vol.30(6), pp.885-895.

42.Tsai C.J.,Perng S.B., and Chiou S.F., 2000, “Use of two different acidic aerosol samplers to measure acidic aerosols in Hsinchu, Taiwan,” Air and Waste ManageAssociation , vol 50, pp.2120-2128.

43.Timothy B.J.,Andrew J.S., and Geraldine E.J.,2006, “Levoglucosan as an atmospheric tracer for woodsmoke” , Atmosphere Environment ,vol.40, iss.27,pp.5316-5321

44.Ueda H., Takemeto T., Kim Y. P. and Sha W., 2000,“Behaviors of volatile inorganic components in urban aerosols”, Atmospheric Environment, vol.34, pp. 353-361.

45.Wang Q.Q.,Shao M.,Liu Y., William K., Paul G., Li X., Liu Y., and Lu S.,2007, “Impact of biomass burning on urban air quality estimated by organic tracers: Guangzhou and Beijing as cases”, Atmospheric Environment, vol.41, pp. 8380-8390.

46.Xiao Y.Y., Lee T., Ayres B., Sonia M. K., Malm W., Collett J.,2006, “Loss of fine particle ammonium from denuded nylon filters”, Atmospheric Environment, vol.40, pp.4797-4807.

47.Yao X , C. K. Chan, M. Fang S. Cadle, T. Chan, P. Mulawa, K. He, and B. Ye, 2002, “The water-soluble ionic composition of PM2.5 in Shanghai and Beijing, China.” Atmospheric Environment Vol. 36 , pp.4223-4234.

48.Zdrahal Z., Oliveira J , Vermeylen R, Claeys M, and Maenhaut W ,2002, “Improved method for Quantifying levoglucosan and related monosaccharide anhydrides in atmospheric aerosol and application to samples from urban and tropical locations. ”Environmental Science and technology. Vol.36 ,pp747-753

49.王秋森,1983,“氣懸膠技術學”,國立台灣大學醫學院出版委員會,台北。

50.張烴、劉咸德、董樹屏、祁輝、Cachier H, Claeys M,2006, “生物質燃燒顆粒示踪化合物的測定和應用”,岩礦測試,第二十五卷,107-113 頁.

51.丁偉諭,2003 ,“台中都會區酸性氣體空氣污染物之季節性變化”,國立中興大學環境工程學系,碩士論文,台中。

52.蔡瀛逸,1999,“台灣中部都會及沿海地區能見度與大氣氣膠化學特性關係之研究”,國立中興大學環境工程研究所博士論文,台中。

53.榮建誠,2007, “都會區高污染大氣中亞硝酸異相生成機制之探討”,國
立中興大學環境工程學系,碩士論文,台中。

54.陳秋吟,2008, “臭氧事件日不同時時段硫酸鹽、硝酸鹽和酸鹼性氣體特性及其影響因子之探討”,國立中興大學環境工程學系,碩士論文,台中。

55.林建利,2012,“稻作種類 Chamber 燃燒粒子特徵暨碳排放之研究”,國立雲林科技大學環境與安全衛生研究所,碩士論文。

56.林暐翔,2005,“大氣中氨氣及銨鹽微粒的量測與特性分析”,國立中興大學環境工程研究所博士論文。

57.李經民,2010,“稻作生質燃燒源 Chamber 脫水醣排放特徵與燃燒條件影響之研究”,國科會報告 ( NSC 98-2221-E-224-005 )。

58.張艮輝,2004,“中部空品區空氣品質改善效益與地區因素之關聯性研究- 子計畫:空氣品質改善效益與氣象地形因素關係之量化評析-空氣品質模式之模擬分析”,國科會報告 (NSC 93-EPA-Z-224-001) 。

59.許旭亨、林桑羽、王俊凱、鄧亦翔、李經民,2012,“台灣露天燃燒常見物種粒子排放特徵暨碳排放之研究”,2012 International Conference on Aerosol Science and Technology。

60.郭正傑,2007,“南部懸浮微粒超級測站之自動監測儀器與手動方法比對”,國立成功大學環境工程研究所,碩士論文。

61.鄭曼婷、丁偉諭、李蔚德、蘇怡如,2003,“農廢燃燒期間空氣污染物的化學組成和粒徑分佈”,第二十屆年空氣污染控制技術研討會論文專輯,pp. 3-73。

62.廖珮妤,2010,“利用燃燒室探討稻作生質燃燒煙塵脫水醣及其排放特徵之研究”,國立雲林科技大學環境與安全衛生工程所,碩士論文。

63.行政環境保護署空氣品質監測網http://taqm.epa.gov.tw/taqm/zh-tw/EpbDataHourly.aspx

64.行政環境保護署空氣品質GIS系統
http://210.69.101.63/gis/

65.行政院農業委員會農糧署
http://www.afa.gov.tw/

QRCODE
 
 
 
 
 
                                                                                                                                                                                                                                                                                                                                                                                                               
第一頁 上一頁 下一頁 最後一頁 top
無相關期刊